EP4052318A1 - Solid oxide cell stack with a pressure difference between anode and cathode compartments - Google Patents

Solid oxide cell stack with a pressure difference between anode and cathode compartments

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Publication number
EP4052318A1
EP4052318A1 EP20786571.8A EP20786571A EP4052318A1 EP 4052318 A1 EP4052318 A1 EP 4052318A1 EP 20786571 A EP20786571 A EP 20786571A EP 4052318 A1 EP4052318 A1 EP 4052318A1
Authority
EP
European Patent Office
Prior art keywords
solid oxide
cell stack
interconnects
oxide cell
stack according
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Pending
Application number
EP20786571.8A
Other languages
German (de)
French (fr)
Inventor
Rainer Küngas
Thomas Heiredal-Clausen
Bengt Peter Gustav Blennow
Tobias Holt NØRBY
Jeppe Rass-Hansen
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Topsoe AS
Original Assignee
Haldor Topsoe AS
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Haldor Topsoe AS filed Critical Haldor Topsoe AS
Publication of EP4052318A1 publication Critical patent/EP4052318A1/en
Pending legal-status Critical Current

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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/02—Details
    • H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
    • H01M8/0247—Collectors; Separators, e.g. bipolar separators; Interconnectors characterised by the form
    • H01M8/0254—Collectors; Separators, e.g. bipolar separators; Interconnectors characterised by the form corrugated or undulated
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/02—Details
    • H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
    • H01M8/0247—Collectors; Separators, e.g. bipolar separators; Interconnectors characterised by the form
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/24—Grouping of fuel cells, e.g. stacking of fuel cells
    • H01M8/241—Grouping of fuel cells, e.g. stacking of fuel cells with solid or matrix-supported electrolytes
    • H01M8/2425—High-temperature cells with solid electrolytes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/02—Details
    • H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
    • H01M8/0204—Non-porous and characterised by the material
    • H01M8/0223—Composites
    • H01M8/0228—Composites in the form of layered or coated products
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/02—Details
    • H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
    • H01M8/023—Porous and characterised by the material
    • H01M8/0236—Glass; Ceramics; Cermets
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/02—Details
    • H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
    • H01M8/0247—Collectors; Separators, e.g. bipolar separators; Interconnectors characterised by the form
    • H01M8/0256—Vias, i.e. connectors passing through the separator material
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/02—Details
    • H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
    • H01M8/0258—Collectors; Separators, e.g. bipolar separators; Interconnectors characterised by the configuration of channels, e.g. by the flow field of the reactant or coolant
    • H01M8/026—Collectors; Separators, e.g. bipolar separators; Interconnectors characterised by the configuration of channels, e.g. by the flow field of the reactant or coolant characterised by grooves, e.g. their pitch or depth
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
    • H01M8/04082—Arrangements for control of reactant parameters, e.g. pressure or concentration
    • H01M8/04089—Arrangements for control of reactant parameters, e.g. pressure or concentration of gaseous reactants
    • H01M8/04104—Regulation of differential pressures
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
    • H01M8/04298—Processes for controlling fuel cells or fuel cell systems
    • H01M8/04313—Processes for controlling fuel cells or fuel cell systems characterised by the detection or assessment of variables; characterised by the detection or assessment of failure or abnormal function
    • H01M8/0432—Temperature; Ambient temperature
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
    • H01M8/04298—Processes for controlling fuel cells or fuel cell systems
    • H01M8/04313—Processes for controlling fuel cells or fuel cell systems characterised by the detection or assessment of variables; characterised by the detection or assessment of failure or abnormal function
    • H01M8/0438—Pressure; Ambient pressure; Flow
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
    • H01M8/04298—Processes for controlling fuel cells or fuel cell systems
    • H01M8/04313—Processes for controlling fuel cells or fuel cell systems characterised by the detection or assessment of variables; characterised by the detection or assessment of failure or abnormal function
    • H01M8/0438—Pressure; Ambient pressure; Flow
    • H01M8/04432—Pressure differences, e.g. between anode and cathode
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/10—Fuel cells with solid electrolytes
    • H01M8/12—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/10—Fuel cells with solid electrolytes
    • H01M8/12—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte
    • H01M2008/1293—Fuel cells with solid oxide electrolytes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2300/00—Electrolytes
    • H01M2300/0017—Non-aqueous electrolytes
    • H01M2300/0065—Solid electrolytes
    • H01M2300/0068—Solid electrolytes inorganic
    • H01M2300/0071—Oxides
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/50—Fuel cells

Definitions

  • the invention relates to a solid oxide cell (SOC) stack, in particular a solid oxide fuel cell (SOFC) unit or a solid oxide electrolysis cell (SOEC) unit, in particular for a SOC stack with a pressure difference between the fuel- compartments of the SOC units and the oxy-compartments of the SOC units stacked upon each other to form a SOC stack.
  • SOC solid oxide cell
  • SOFC solid oxide fuel cell
  • SOEC solid oxide electrolysis cell
  • the invention proposes a design for a solid oxide cell (SOC) stack that is mechanically robust towards operation with a pressure difference between the fuel- and oxy- compartments of the stack. This is achieved by choosing the distance between contact points/ribs on the low-pressure side of the SOC such that the maximum tensile stress expe rienced by the SOC due to the applied pressure difference between the two sides of the cell is significantly below the Weibull strength of the SOC.
  • SOC solid oxide cell
  • Solid oxide cells typically comprise of layers of ce ramic and metal-ceramic composite (cermet) materials. Re gardless of the chosen cell geometry (tubular, planar, in tegrated planar, etc.), one of the cell layers is typically considerably thicker than other layers and provides mechan ical support for the thinner layers. For example, in elec trolyte-supported cells, a gas-tight electrolyte layer (consisting, e.g. of stabilized zirconia or doped ceria) is typically the thickest layer in the cell. The mechanical strength of such a cell is determined by the properties of electrolyte.
  • the fuel- electrode is the thickest layer in the cell and the mechan ical properties of the cell are determined by the fuel- electrode.
  • the fuel-electrode is typically a cermet materi al, comprising metallic Ni and an oxygen ion-conducting ma terial, such as stabilized zirconia or doped ceria. Due to the use of ceramic materials, SOCs are brittle. A material is considered brittle, if, when subjected to stress, it fractures or fails with little or no plastic deformation. A ductile material, in contrast, is able to undergo signifi cant plastic deformation before rupture, when subjected to stress.
  • SOCs To increase the output of an SOC unit, several SOCs are connected in series to form an SOC stack.
  • the mechanical failure of a single SOC in a stack usually leads to the failure of the entire stack.
  • the higher the number of cells in a stack the lower the allowable failure rate of cells. For example, if the cell failure rate is 1/1000, then the corresponding stack failure rate is 1/100 for a 10-cell stack, but 1/10 for 100-cell stack.
  • the strength of the cell character ized typically in terms of Weibull strength and Weibull modulus, should be maximized.
  • the strength of ceramic materials is not an intrinsic prop erty, but depends on the size and distribution of flaws, which arise during the manufacturing process and act as stress concentrators.
  • Weibull strength and Weibull modulus can be estimated using a number of methods, such as ball-on-ring, 4-point-bending, ring-on-ring, etc.
  • solid oxide cells are fed with reactant gases.
  • the fuel-side of the SOC could be fed with a fuel, such as hydrogen, methane, natural gas, syngas, etc.
  • the oxy-side of the SOC could be fed with an oxi dant, such as air.
  • the fuel-side of the SOC could be fed with e.g. steam and/or carbon dioxide, while a flush gas, such as oxygen, steam, nitrogen or carbon dioxide could be fed to the oxy-side.
  • the pressure of gases on each side of the SOC can, in prin cipal, be chosen freely. However, due to the brittleness of SOCs, it is common practice in the field to completely avoid pressure differences from occurring during operation. However, operation of SOC stacks with a non-zero pressure difference between the fuel- and oxy-side of the stack, if possible, would have significant advantages.
  • US6902840 B2 teaches that it is desirable to minimize the pressure differential of the gases passing through the anode and cathode sides of the stacks and pro poses the use of a mixer/educator to operate and mix said exhaust fuel gas and supply of oxidant gas such that the difference between the pressure of said exhaust fuel gas at the exit of the anode-side and the pressure of the oxidant gas at the inlet of the cathode-side is reduced.
  • US 2011/0027683 A1 proposes the use of seal materials with serpentine seal geometry to avoid seal failure, electrolyte failure (stress induced fracturing of electrolyte sheet wrinkles, buckling or corrugation), or device failure due to differential gas pressure and inter actions between the device, the seal and the cell support frame.
  • the invention proposes a stack design, where the distance between contact points/ribs on the low-pressure side of the SOC are chosen such that the maximum tensile stress experienced by the SOC due to the applied pressure difference between the two sides of the cell is signifi cantly below the Weibull strength of the SOC.
  • Transient pressure differences between the compartments can occur during stack operation, e.g. when the flow rates are changed or when a blower/compressor is started/stopped.
  • a stack design that is robust towards such transient pressure differences would allow cheaper pressure control equipment to be used for monitoring/controlling the inlet pressures for oxy- and fuel compartments.
  • the invention would minimize the need for buffer tanks (e.g. for steam), which are often used to smoothen out transient pressure differences.
  • the fuel-side feed gas for example steam, CO 2 , or a mixture of thereof
  • the fuel-side feed gas for example steam, CO 2 , or a mixture of thereof
  • the resulting prod uct 3 ⁇ 4, CO, or syngas
  • an additional compressor is needed for pressurizing the oxy- side gas prior to entering the stack.
  • the proposed inven tion would eliminate the need for the oxy-side compressor and would thus involve significant cost savings, both in CAPEX and OPEX. Additionally, in a stack built according to the invention, the inlet pressures of the oxy- and fuel- side gases need not be matched exactly, which simplifies the system design and eliminates the need for buffer tanks.
  • the fuel-side feed gas e.g. 3 ⁇ 4, CH 4 , natural gas, etc.
  • the fuel-side feed gas e.g. 3 ⁇ 4, CH 4 , natural gas, etc.
  • Solid Oxide Cell stack comprising a plurality of stacked cell units as known in the art.
  • Each unit comprises a solid oxide cell in a cell layer and an interconnect in an inter connect layer.
  • One interconnect layer separates one cell unit from the adjacent cell unit in the cell stack and thus provides a gas barrier between the cell units.
  • the inter connect also serves the purpose of providing gas flow chan nels and electrical contact between the cell units.
  • each interconnect comprising one or more protrud ing contact areas on a first side and one or more protrud ing contact areas on a second side of the interconnect adapted to provide mechanical and electrical contact be tween interconnects and solid oxide cells as well as gas flow channels in between the contact areas on both the first and the second side of the interconnect.
  • the contact areas on both sides of each in terconnect protrudes at least relative to the bottom part of the gas flow channels.
  • each solid oxide cell has a high-pressure side facing the first side of an adjacent interconnect and a low-pressure side facing a second side of an adjacent interconnect.
  • the maximum distance between two adjacent edges of the contact areas on the second side of the interconnects is 2.5 mm, whereby also the tensile stress experienced by the SOC due to the applied pressure difference between the first and the second side of the interconnect also has a maximum which is related to the applied pressure and the distance between the two adjacent edges of the contact areas.
  • the interconnect is according to this invention designed to provide a maximum tensile stress experienced by the SOC by means of a maximum distance be tween two adjacent edges of the contact areas on the second side of the interconnects.
  • said maximum difference can be 0.3 mm, 0.4 mm, 0.5 mm, 0.6 mm, 0.7 mm, 0.8 mm, 0.9 mm, 1.0 mm, 1.2 mm, 1.5 mm, 1.8 mm or 2.5 mm depending on the mentioned operation conditions and SOC strength.
  • the dis cussed maximum distance between two adjacent edges of the contact areas on the first side of the interconnects is the same or larger than the maximum distance between two adja cent edges of the contact areas on the second side of the interconnects.
  • the interconnect design may be tailored to the different process parameters and tensile stress which are at either side of the interconnect. I.e. the distance between two adjacent edges of the contact are as on one side is suited for the pressure and thus the stress on that side whereas the pressure and stress on the other side may be different and the discussed distance on that side may therefore also differ to meet the strength demands .
  • the interconnects of the SOC stack each has an area of between 15 cm 2 and 10000 cm 2 , preferably between 64 and 500 cm 2 .
  • the cell units may be ceramic in an embodiment of the in vention.
  • the interconnects may comprise one or more intermediate contact enhancing layers.
  • the SOC stack is a Solid Oxide Electrolysis cell stack.
  • the pressure difference between the high-pressure side and the low- pressure side is minimum 300 mBar.
  • said pressure difference is minimum 1 Bar, preferably minimum 5 Bar or even minimum 15 Bar. It is to be understood that the maximum distance between two ad jacent edges of the contact areas on the second side of the interconnects may vary accordingly such that the higher the pressure difference, the smaller the maximum distance be tween two adjacent edges of said contact areas.
  • Solid Oxide Cell stack comprising a plurality of stacked cell units, each unit comprises a solid oxide cell in a cell layer and an interconnect in an interconnect layer, wherein one interconnect layer separates one cell layer from the adjacent cell layer in the cell stack, each inter connect comprises one or more protruding contact areas on a first side and one or more protruding contact areas on a second side of the interconnect adapted to provide mechani cal and electrical contact between interconnects and solid oxide cells, wherein each solid oxide cell has a high-pressure side fac ing the first side of an adjacent interconnect and a low- pressure side facing a second side of an adjacent intercon nect and wherein the maximum distance between two adjacent edges of the contact areas on the second side of the inter connects is 2.5 mm.
  • Solid Oxide Cell stack according to feature 1 wherein the maximum distance between two adjacent edges of the con tact areas on the second side of the interconnects is 2.0 mm.
  • Solid Oxide Cell stack according to feature 1 wherein the maximum distance between two adjacent edges of the con- tact areas on the second side of the interconnects is 1.8 mm.
  • Solid Oxide Cell stack according to feature 1 wherein the maximum distance between two adjacent edges of the con tact areas on the second side of the interconnects is 1.5 mm.
  • Solid Oxide Cell stack according to feature 1 wherein the maximum distance between two adjacent edges of the con tact areas on the second side of the interconnects is 1.2 mm.
  • Solid Oxide Cell stack according to feature 1 wherein the maximum distance between two adjacent edges of the con tact areas on the second side of the interconnects is 1.0 mm.
  • Solid Oxide Cell stack according to feature 1 wherein the maximum distance between two adjacent edges of the con tact areas on the second side of the interconnects is 0.9 mm.
  • Solid Oxide Cell stack according to feature 1 wherein the maximum distance between two adjacent edges of the con tact areas on the second side of the interconnects is 0.8 mm.
  • Solid Oxide Cell stack according to feature 1 wherein the maximum distance between two adjacent edges of the con tact areas on the second side of the interconnects is 0.7 mm. 10. Solid Oxide Cell stack according to feature 1, wherein the maximum distance between two adjacent edges of the con tact areas on the second side of the interconnects is 0.6 mm.
  • Solid Oxide Cell stack according to feature 1 wherein the maximum distance between two adjacent edges of the con tact areas on the second side of the interconnects is 0.5 mm.
  • Solid Oxide Cell stack according to feature 1 wherein the maximum distance between two adjacent edges of the con tact areas on the second side of the interconnects is 0.4 mm.
  • Solid Oxide Cell stack according to feature 1 wherein the maximum distance between two adjacent edges of the con tact areas on the second side of the interconnects is 0.3 mm.
  • Solid Oxide Cell stack according to any of the preced ing features, wherein the maximum distance between two ad jacent edges of the contact areas on the first side of the interconnects is the same or larger than the maximum dis tance between two adjacent edges of the contact areas on the second side of the interconnects.
  • Solid Oxide Cell stack according to any of the preced ing features wherein the area of each of the interconnects is between 15 cm 2 and 10000 cm 2 , preferably between 64 and 500 cm 2 . 16. Solid Oxide Cell stack according to any of the preced ing features, wherein the solid oxide cells are ceramic cells.
  • Solid Oxide Cell stack according to any of the preced ing features, wherein the interconnects comprise one or more intermediate contact enhancing layers.
  • Solid Oxide Cell stack according to any of the preced ing features, wherein the Solid Oxide Cell stack is a Solid Oxide Electrolysis cell stack.
  • Solid Oxide Cell stack according to any of the preced ing features, wherein the pressure difference between the high-pressure side and the low-pressure side is minimum 300 mBar.
  • Solid Oxide Cell stack according to any of the preced ing features, wherein the pressure difference between the high-pressure side and the low-pressure side is minimum 1 Bar, preferably minimum 5 Bar, preferably minimum 15 Bar.
  • Solid Oxide Cell stack according to any of the preced ing features, wherein the high-pressure side is a fuel- side.
  • Fig. 1 shows a partial principle side cut of a part of an SOC stack according to an embodiment of the invention.
  • SOC Solid Oxide Cell
  • H High pressure side
  • L low pressure side
  • Interconnects 102 separating each SOC from the next in the cell stack.
  • An SOC and one intercon nect each forming a cell unit 103.
  • the high pressure side of the SOC faces a first side of an interconnect and the low pressure side of the SOC faces a second side of the in terconnect.
  • the interconnects comprise protruding contact areas on both the first and the second side of the inter connect.
  • the maximum distance between two adjacent edges of the contact areas on the sec ond side of each interconnect Ml is adapted be 2.5 mm, to support the cell unit.
  • the distance M2 between two adjacent edges of the contact areas on the first side of each inter connect may in an embodiment of the invention be larger than Ml, since the high pressure side of the SOC needs less support than the low pressure side.
  • the high pressure side of the SOC is the fuel side of the SOC.
  • the design of the invention was tested in two short SOC stacks containing 9 single repeat cell units.
  • the distance between the contact points/ribs on the low pressure oxy side was 1.3 mm, and the fuel side was pressurized up to 1.75 bara yielding a pressure difference from fuel to oxy side of up to 750 mbar.
  • the first test was performed in electrolysis mode, with fuel containing 5% hydrogen in steam.
  • the oxy side was flushed with air and kept at ambient pressure (1.013 bara) throughout the test.
  • the inlet gases were heated to 750°C and the stack was installed in a furnace keeping the tem perature around the stack stable at 750°C.
  • the stack was run at a current density of approximately 0.75A/cm2.
  • Below is a table showing the average cell voltage at the chosen operating point with increasing fuel side pressure.
  • the average voltage of the cells decreases as the fuel side pressure increases, which in SOEC mode corresponds to improved performance.
  • the in creased performance at this operating point corresponds to a reduced power consumption of a little more than 1%.
  • the second test was performed in SOFC mode on a fuel of 60% hydrogen and 40% nitrogen. Again, the oxy side was flushed with air and kept at ambient pressure (1.013 bara) through out the test. The inlet gases were heated to 700°C and the SOC stack was installed in a furnace keeping the tempera ture around the SOC stack stable at 700°C. The SOC stack was run at a current density of approximately 0.28A/cm2. Below is a table showing the average cell voltage at the chosen operating point with increasing fuel side pressure.
  • the average voltage of the cells increases as the fuel side pressure increases, which in SOFC mode corresponds to improved performance.
  • the in creased performance at this operating point corresponds to an increase in power output of roughly 0.6%.

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Abstract

A SOC stack has interconnects with a maximum distance between the contact points which are designed to compensate for pressure difference between one side of the interconnect to the other side.

Description

Solid oxide cell stack with a pressure difference between anode and cathode compartments
FIELD OF THE INVENTION
The invention relates to a solid oxide cell (SOC) stack, in particular a solid oxide fuel cell (SOFC) unit or a solid oxide electrolysis cell (SOEC) unit, in particular for a SOC stack with a pressure difference between the fuel- compartments of the SOC units and the oxy-compartments of the SOC units stacked upon each other to form a SOC stack.
BACKGROUND OF THE INVENTION
The invention proposes a design for a solid oxide cell (SOC) stack that is mechanically robust towards operation with a pressure difference between the fuel- and oxy- compartments of the stack. This is achieved by choosing the distance between contact points/ribs on the low-pressure side of the SOC such that the maximum tensile stress expe rienced by the SOC due to the applied pressure difference between the two sides of the cell is significantly below the Weibull strength of the SOC.
Solid oxide cells (SOC) typically comprise of layers of ce ramic and metal-ceramic composite (cermet) materials. Re gardless of the chosen cell geometry (tubular, planar, in tegrated planar, etc.), one of the cell layers is typically considerably thicker than other layers and provides mechan ical support for the thinner layers. For example, in elec trolyte-supported cells, a gas-tight electrolyte layer (consisting, e.g. of stabilized zirconia or doped ceria) is typically the thickest layer in the cell. The mechanical strength of such a cell is determined by the properties of electrolyte. In fuel-electrode supported cells, the fuel- electrode is the thickest layer in the cell and the mechan ical properties of the cell are determined by the fuel- electrode. The fuel-electrode is typically a cermet materi al, comprising metallic Ni and an oxygen ion-conducting ma terial, such as stabilized zirconia or doped ceria. Due to the use of ceramic materials, SOCs are brittle. A material is considered brittle, if, when subjected to stress, it fractures or fails with little or no plastic deformation. A ductile material, in contrast, is able to undergo signifi cant plastic deformation before rupture, when subjected to stress.
To increase the output of an SOC unit, several SOCs are connected in series to form an SOC stack. The mechanical failure of a single SOC in a stack usually leads to the failure of the entire stack. The higher the number of cells in a stack, the lower the allowable failure rate of cells. For example, if the cell failure rate is 1/1000, then the corresponding stack failure rate is 1/100 for a 10-cell stack, but 1/10 for 100-cell stack. In order to achieve a low cell failure rate, the strength of the cell, character ized typically in terms of Weibull strength and Weibull modulus, should be maximized. It should be understood that the strength of ceramic materials is not an intrinsic prop erty, but depends on the size and distribution of flaws, which arise during the manufacturing process and act as stress concentrators. As a result, the probability of fail ure of such samples is statistically distributed and is commonly characterized using the Weibull distribution. The Weibull distribution quantifies the variability of the strength of the samples resulting from a distribution of flaw sizes. According to the distribution, the probability of failure, P is given as Pf = 1 - exp [-(s/s0) m], where s is the applied stress, sois the Weibull strength, and m is the Weibull modulus. Weibull strength and Weibull modulus can be estimated using a number of methods, such as ball-on-ring, 4-point-bending, ring-on-ring, etc.
During operation, solid oxide cells are fed with reactant gases. For example, when SOC is operating in solid oxide fuel cell mode, the fuel-side of the SOC could be fed with a fuel, such as hydrogen, methane, natural gas, syngas, etc., and the oxy-side of the SOC could be fed with an oxi dant, such as air. When SOC is operating in solid oxide electrolysis mode, the fuel-side of the SOC could be fed with e.g. steam and/or carbon dioxide, while a flush gas, such as oxygen, steam, nitrogen or carbon dioxide could be fed to the oxy-side.
The pressure of gases on each side of the SOC can, in prin cipal, be chosen freely. However, due to the brittleness of SOCs, it is common practice in the field to completely avoid pressure differences from occurring during operation. However, operation of SOC stacks with a non-zero pressure difference between the fuel- and oxy-side of the stack, if possible, would have significant advantages.
For example, US6902840 B2 teaches that it is desirable to minimize the pressure differential of the gases passing through the anode and cathode sides of the stacks and pro poses the use of a mixer/educator to operate and mix said exhaust fuel gas and supply of oxidant gas such that the difference between the pressure of said exhaust fuel gas at the exit of the anode-side and the pressure of the oxidant gas at the inlet of the cathode-side is reduced.
In another example, US 2011/0027683 A1 proposes the use of seal materials with serpentine seal geometry to avoid seal failure, electrolyte failure (stress induced fracturing of electrolyte sheet wrinkles, buckling or corrugation), or device failure due to differential gas pressure and inter actions between the device, the seal and the cell support frame.
SUMMARY OF THE INVENTION
Now, it has turned out that it is possible to operate an SOC stack with a pressure difference between the fuel- and oxy-side of the stack by providing sufficient mechanical support to the low-pressure side of the SOC. More specifi cally, the invention proposes a stack design, where the distance between contact points/ribs on the low-pressure side of the SOC are chosen such that the maximum tensile stress experienced by the SOC due to the applied pressure difference between the two sides of the cell is signifi cantly below the Weibull strength of the SOC.
Being able to operate an SOC stack with either a steady- state or transient pressure difference between the fuel- and oxy-compartments has several advantages. Transient pressure differences between the compartments can occur during stack operation, e.g. when the flow rates are changed or when a blower/compressor is started/stopped. A stack design that is robust towards such transient pressure differences would allow cheaper pressure control equipment to be used for monitoring/controlling the inlet pressures for oxy- and fuel compartments. Additionally, the invention would minimize the need for buffer tanks (e.g. for steam), which are often used to smoothen out transient pressure differences.
In solid oxide electrolysis mode, the fuel-side feed gas (for example steam, CO2, or a mixture of thereof) is typi cally provided in pressurized state and the resulting prod uct (¾, CO, or syngas) should be pressurized. It is there fore desirable to operate the fuel-side compartment of the stack at an elevated pressure to avoid both an additional decompression of gases prior to entering the stack and a recompression of product gases after leaving the stack. Ac cording to the state-of-the-art, this implies that the oxy- side compartment of the stack needs to be pressurized to the same pressure as the fuel-side compartment. Hence, an additional compressor is needed for pressurizing the oxy- side gas prior to entering the stack. The proposed inven tion would eliminate the need for the oxy-side compressor and would thus involve significant cost savings, both in CAPEX and OPEX. Additionally, in a stack built according to the invention, the inlet pressures of the oxy- and fuel- side gases need not be matched exactly, which simplifies the system design and eliminates the need for buffer tanks. In solid oxide fuel cell mode, the fuel-side feed gas (e.g. ¾, CH4, natural gas, etc.) is often provided in pressur ized state and the one (the other product being electrici ty) resulting product gas (CO2, steam) can be advantageous ly used to drive a gas turbine, if pressurized. It is therefore desirable to operate the fuel-side compartment of the stack at an elevated pressure to avoid both an addi tional decompression of gases prior to entering the stack and a recompression of product gases after leaving the stack. According to the state-of-the-art, this implies that the oxy-side compartment of the stack needs to be pressur ized to the same pressure as the fuel-side compartment. Hence, an additional compressor is needed for pressurizing the oxy-side gas prior to entering the stack. The proposed invention would eliminate the need for the oxy-side com pressor and would thus involve significant cost savings, both in CAPEX and OPEX.
More specifically, the present invention solves the above discussed problems according to the claims by providing a Solid Oxide Cell stack comprising a plurality of stacked cell units as known in the art. Each unit comprises a solid oxide cell in a cell layer and an interconnect in an inter connect layer. One interconnect layer separates one cell unit from the adjacent cell unit in the cell stack and thus provides a gas barrier between the cell units. The inter connect also serves the purpose of providing gas flow chan nels and electrical contact between the cell units. This is solved by each interconnect comprising one or more protrud ing contact areas on a first side and one or more protrud ing contact areas on a second side of the interconnect adapted to provide mechanical and electrical contact be tween interconnects and solid oxide cells as well as gas flow channels in between the contact areas on both the first and the second side of the interconnect. It is to be understood that the contact areas on both sides of each in terconnect protrudes at least relative to the bottom part of the gas flow channels. Particular for this invention, each solid oxide cell has a high-pressure side facing the first side of an adjacent interconnect and a low-pressure side facing a second side of an adjacent interconnect. The maximum distance between two adjacent edges of the contact areas on the second side of the interconnects is 2.5 mm, whereby also the tensile stress experienced by the SOC due to the applied pressure difference between the first and the second side of the interconnect also has a maximum which is related to the applied pressure and the distance between the two adjacent edges of the contact areas.
Hence, for a given SOC unit with given strength and for given operation condition, the interconnect is according to this invention designed to provide a maximum tensile stress experienced by the SOC by means of a maximum distance be tween two adjacent edges of the contact areas on the second side of the interconnects. Accordingly, in further embodi ments of the invention, with different applications regard ing SOC strength and/or pressure difference, said maximum difference can be 0.3 mm, 0.4 mm, 0.5 mm, 0.6 mm, 0.7 mm, 0.8 mm, 0.9 mm, 1.0 mm, 1.2 mm, 1.5 mm, 1.8 mm or 2.5 mm depending on the mentioned operation conditions and SOC strength. According to another embodiment of the invention, the dis cussed maximum distance between two adjacent edges of the contact areas on the first side of the interconnects is the same or larger than the maximum distance between two adja cent edges of the contact areas on the second side of the interconnects. In this manner, the interconnect design may be tailored to the different process parameters and tensile stress which are at either side of the interconnect. I.e. the distance between two adjacent edges of the contact are as on one side is suited for the pressure and thus the stress on that side whereas the pressure and stress on the other side may be different and the discussed distance on that side may therefore also differ to meet the strength demands .
In a further embodiment of the invention, the interconnects of the SOC stack each has an area of between 15 cm2 and 10000 cm2, preferably between 64 and 500 cm2.
The cell units may be ceramic in an embodiment of the in vention. Also, the interconnects may comprise one or more intermediate contact enhancing layers. In a particular em bodiment of the invention, the SOC stack is a Solid Oxide Electrolysis cell stack.
According to an embodiment of the invention, the pressure difference between the high-pressure side and the low- pressure side is minimum 300 mBar. In a further embodiment of the invention, said pressure difference is minimum 1 Bar, preferably minimum 5 Bar or even minimum 15 Bar. It is to be understood that the maximum distance between two ad jacent edges of the contact areas on the second side of the interconnects may vary accordingly such that the higher the pressure difference, the smaller the maximum distance be tween two adjacent edges of said contact areas.
FEATURES OF THE INVENTION
1. Solid Oxide Cell stack comprising a plurality of stacked cell units, each unit comprises a solid oxide cell in a cell layer and an interconnect in an interconnect layer, wherein one interconnect layer separates one cell layer from the adjacent cell layer in the cell stack, each inter connect comprises one or more protruding contact areas on a first side and one or more protruding contact areas on a second side of the interconnect adapted to provide mechani cal and electrical contact between interconnects and solid oxide cells, wherein each solid oxide cell has a high-pressure side fac ing the first side of an adjacent interconnect and a low- pressure side facing a second side of an adjacent intercon nect and wherein the maximum distance between two adjacent edges of the contact areas on the second side of the inter connects is 2.5 mm.
2. Solid Oxide Cell stack according to feature 1, wherein the maximum distance between two adjacent edges of the con tact areas on the second side of the interconnects is 2.0 mm.
3. Solid Oxide Cell stack according to feature 1, wherein the maximum distance between two adjacent edges of the con- tact areas on the second side of the interconnects is 1.8 mm.
4. Solid Oxide Cell stack according to feature 1, wherein the maximum distance between two adjacent edges of the con tact areas on the second side of the interconnects is 1.5 mm.
5. Solid Oxide Cell stack according to feature 1, wherein the maximum distance between two adjacent edges of the con tact areas on the second side of the interconnects is 1.2 mm.
6. Solid Oxide Cell stack according to feature 1, wherein the maximum distance between two adjacent edges of the con tact areas on the second side of the interconnects is 1.0 mm.
7. Solid Oxide Cell stack according to feature 1, wherein the maximum distance between two adjacent edges of the con tact areas on the second side of the interconnects is 0.9 mm.
8. Solid Oxide Cell stack according to feature 1, wherein the maximum distance between two adjacent edges of the con tact areas on the second side of the interconnects is 0.8 mm.
9. Solid Oxide Cell stack according to feature 1, wherein the maximum distance between two adjacent edges of the con tact areas on the second side of the interconnects is 0.7 mm. 10. Solid Oxide Cell stack according to feature 1, wherein the maximum distance between two adjacent edges of the con tact areas on the second side of the interconnects is 0.6 mm.
11. Solid Oxide Cell stack according to feature 1, wherein the maximum distance between two adjacent edges of the con tact areas on the second side of the interconnects is 0.5 mm.
12. Solid Oxide Cell stack according to feature 1, wherein the maximum distance between two adjacent edges of the con tact areas on the second side of the interconnects is 0.4 mm.
13. Solid Oxide Cell stack according to feature 1, wherein the maximum distance between two adjacent edges of the con tact areas on the second side of the interconnects is 0.3 mm.
14. Solid Oxide Cell stack according to any of the preced ing features, wherein the maximum distance between two ad jacent edges of the contact areas on the first side of the interconnects is the same or larger than the maximum dis tance between two adjacent edges of the contact areas on the second side of the interconnects.
15. Solid Oxide Cell stack according to any of the preced ing features, wherein the area of each of the interconnects is between 15 cm2 and 10000 cm2, preferably between 64 and 500 cm2. 16. Solid Oxide Cell stack according to any of the preced ing features, wherein the solid oxide cells are ceramic cells.
17. Solid Oxide Cell stack according to any of the preced ing features, wherein the interconnects comprise one or more intermediate contact enhancing layers.
18. Solid Oxide Cell stack according to any of the preced ing features, wherein the Solid Oxide Cell stack is a Solid Oxide Electrolysis cell stack.
19. Solid Oxide Cell stack according to any of the preced ing features, wherein the pressure difference between the high-pressure side and the low-pressure side is minimum 300 mBar.
20. Solid Oxide Cell stack according to any of the preced ing features, wherein the pressure difference between the high-pressure side and the low-pressure side is minimum 1 Bar, preferably minimum 5 Bar, preferably minimum 15 Bar.
21. Solid Oxide Cell stack according to any of the preced ing features, wherein the high-pressure side is a fuel- side. DRAWING
In the following an embodiment of the invention will be ex plained with reference to Fig. 1, which shows a partial principle side cut of a part of an SOC stack according to an embodiment of the invention.
A part of an Solid Oxide Cell (SOC) 101 is shown with a high pressure side, H and a low pressure side L. It is to be understood that several SOCs are stacked in layers in the SOC stack, with Interconnects, 102 separating each SOC from the next in the cell stack. An SOC and one intercon nect each forming a cell unit 103. The high pressure side of the SOC faces a first side of an interconnect and the low pressure side of the SOC faces a second side of the in terconnect. The interconnects comprise protruding contact areas on both the first and the second side of the inter connect. According to the invention, the maximum distance between two adjacent edges of the contact areas on the sec ond side of each interconnect Ml, is adapted be 2.5 mm, to support the cell unit. The distance M2 between two adjacent edges of the contact areas on the first side of each inter connect may in an embodiment of the invention be larger than Ml, since the high pressure side of the SOC needs less support than the low pressure side. In a further embodiment of the invention, the high pressure side of the SOC is the fuel side of the SOC. EXAMPLES
The design of the invention was tested in two short SOC stacks containing 9 single repeat cell units. The distance between the contact points/ribs on the low pressure oxy side was 1.3 mm, and the fuel side was pressurized up to 1.75 bara yielding a pressure difference from fuel to oxy side of up to 750 mbar.
The first test was performed in electrolysis mode, with fuel containing 5% hydrogen in steam. The oxy side was flushed with air and kept at ambient pressure (1.013 bara) throughout the test. The inlet gases were heated to 750°C and the stack was installed in a furnace keeping the tem perature around the stack stable at 750°C. The stack was run at a current density of approximately 0.75A/cm2. Below is a table showing the average cell voltage at the chosen operating point with increasing fuel side pressure.
As seen from the table, the average voltage of the cells decreases as the fuel side pressure increases, which in SOEC mode corresponds to improved performance. The in creased performance at this operating point corresponds to a reduced power consumption of a little more than 1%. The second test was performed in SOFC mode on a fuel of 60% hydrogen and 40% nitrogen. Again, the oxy side was flushed with air and kept at ambient pressure (1.013 bara) through out the test. The inlet gases were heated to 700°C and the SOC stack was installed in a furnace keeping the tempera ture around the SOC stack stable at 700°C. The SOC stack was run at a current density of approximately 0.28A/cm2. Below is a table showing the average cell voltage at the chosen operating point with increasing fuel side pressure.
As seen from the table, the average voltage of the cells increases as the fuel side pressure increases, which in SOFC mode corresponds to improved performance. The in creased performance at this operating point corresponds to an increase in power output of roughly 0.6%.

Claims

CLAIMS .
1. Solid Oxide Cell stack comprising a plurality of stacked cell units, each unit comprises a solid oxide cell in a cell layer and an interconnect in an interconnect layer, wherein one interconnect layer separates one cell layer from the adjacent cell layer in the cell stack, each inter connect comprises one or more protruding contact areas on a first side and one or more protruding contact areas on a second side of the interconnect adapted to provide mechani cal and electrical contact between interconnects and solid oxide cells, wherein each solid oxide cell has a high-pressure side fac ing the first side of an adjacent interconnect and a low- pressure side facing a second side of an adjacent intercon nect and wherein the maximum distance between two adjacent edges of the contact areas on the second side of the inter connects is 2.5 mm.
2. Solid Oxide Cell stack according to claim 1, wherein the maximum distance between two adjacent edges of the contact areas on the second side of the interconnects is 2.0 mm.
3. Solid Oxide Cell stack according to claim 1, wherein the maximum distance between two adjacent edges of the contact areas on the second side of the interconnects is 1.8 mm.
4. Solid Oxide Cell stack according to claim 1, wherein the maximum distance between two adjacent edges of the contact areas on the second side of the interconnects is 1.5 mm.
5. Solid Oxide Cell stack according to claim 1, wherein the maximum distance between two adjacent edges of the contact areas on the second side of the interconnects is 1.2 mm.
6. Solid Oxide Cell stack according to claim 1, wherein the maximum distance between two adjacent edges of the contact areas on the second side of the interconnects is 1.0 mm.
7. Solid Oxide Cell stack according to claim 1, wherein the maximum distance between two adjacent edges of the contact areas on the second side of the interconnects is 0.9 mm.
8. Solid Oxide Cell stack according to claim 1, wherein the maximum distance between two adjacent edges of the contact areas on the second side of the interconnects is 0.8 mm.
9. Solid Oxide Cell stack according to claim 1, wherein the maximum distance between two adjacent edges of the contact areas on the second side of the interconnects is 0.7 mm.
10. Solid Oxide Cell stack according to claim 1, wherein the maximum distance between two adjacent edges of the con tact areas on the second side of the interconnects is 0.6 mm.
11. Solid Oxide Cell stack according to claim 1, wherein the maximum distance between two adjacent edges of the con tact areas on the second side of the interconnects is 0.5 mm.
12. Solid Oxide Cell stack according to claim 1, wherein the maximum distance between two adjacent edges of the con- tact areas on the second side of the interconnects is 0.4 mm.
13. Solid Oxide Cell stack according to claim 1, wherein the maximum distance between two adjacent edges of the con tact areas on the second side of the interconnects is 0.3 mm.
14. Solid Oxide Cell stack according to any of the preced ing claims, wherein the maximum distance between two adja cent edges of the contact areas on the first side of the interconnects is the same or larger than the maximum dis tance between two adjacent edges of the contact areas on the second side of the interconnects.
15. Solid Oxide Cell stack according to any of the preced ing claims, wherein the area of each of the interconnects is between 15 cm2 and 10000 cm2, preferably between 64 and 500 cm2.
16. Solid Oxide Cell stack according to any of the preced ing claims, wherein the solid oxide cells are ceramic cells.
17. Solid Oxide Cell stack according to any of the preced ing claims, wherein the interconnects comprise one or more intermediate contact enhancing layers.
18. Solid Oxide Cell stack according to any of the preced ing claims, wherein the Solid Oxide Cell stack is a Solid Oxide Electrolysis cell stack.
19. Solid Oxide Cell stack according to any of the preced ing claims, wherein the pressure difference between the high-pressure side and the low-pressure side is minimum 300 mBar.
20. Solid Oxide Cell stack according to any of the preced ing claims, wherein the pressure difference between the high-pressure side and the low-pressure side is minimum 1 Bar, preferably minimum 5 Bar, preferably minimum 15 Bar.
21. Solid Oxide Cell stack according to any of the preced ing features, wherein the high-pressure side is a fuel- side.
EP20786571.8A 2019-10-28 2020-10-07 Solid oxide cell stack with a pressure difference between anode and cathode compartments Pending EP4052318A1 (en)

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